Component resolved OSL dose response and sensitization of various sedimentary quartz samples

The structure of the linearly modulated optically stimulated luminescence (LM-OSL) signal was studied for four sedimentary quartz samples, collected from different sites around Istanbul, Turkey. Applying a computerized deconvolution analysis to the LM-OSL curves, at least six individual components of first-order kinetics were identified and photoionization cross-section of each component was evaluated. The OSL dose–response curve of each component for each quartz sample was obtained, showing a remarkable differentiation from component to component. The behavior of a highly dosed sample to successive LM-OSL measurements was also studied showing a stable recuperation signal in the position of the “slow” and “medium” components and high resistance to OSL bleaching of the “slow” component. The individual sensitivity of each component as a function of the activation temperature was obtained. The sensitivity of each component was normalized over the respective sensitivity of the glow-peak at 110 °C of quartz in order to investigate the ability of the 110 °C glow-peak to act as a correction factor for all components of the LM-OSL curves examined.     

The slow component of quartz optically stimulated luminescence

The slow component of quartz OSL displays a number of properties that clearly distinguish it from the main (‘rapidly bleachable’) part of the quartz OSL signal traditionally used for dating. These properties include an extremely high thermal stability, dose saturation level and a charge concentration dependence in both signal form and decay rate. The physical mechanism responsible for the slow component is thought at present to involve a direct donor–acceptor recombination component, possibly associated with competing pathways below, and possibly up to, the conduction band. The thermal stability and high dose saturation characteristics of the slow component suggest much potential for long-range dating exists although at present it is uncertain whether difficulties associated with partial resetting may preclude routine use of the slow component for dating sedimentary deposits. A single-aliquot additive dose method was however used to obtain an estimate of D_e from the slow component for an Egyptian quartz sample that was in broad agreement with previous estimates based on the standard multiple-aliquot additive dose method.The slow component is often small in magnitude compared to the initial portion of the quartz OSL decay. However, this is not always the case and for some samples significant inaccuracies in D_e estimation may occur when deriving ages from the initial ‘rapidly bleaching’ portion of the OSL decay if the effect of the slow component is ignored or taken to be constant.     

Relative response of TL and component-resolved OSL to alpha and beta radiations in annealed sedimentary quartz

Knowledge of the relative luminescence response to alpha and beta radiation is very important in TL and OSL dating. In the present study the relative alpha to beta response is studied in a sedimentary quartz sample, previously fired at 900 °C for 1 h, in the dose region between 1 and 128 Gy, for both thermoluminescence (TL) and linearly modulated optically stimulated luminescence (LM – OSL). The LM – OSL measurements were performed at room temperature and at 125 °C. All OSL signals were deconvolved into their individual components. Comparison of OSL curves after alpha and beta irradiation strongly supports that quartz OSL components follow first order kinetics in both cases. In the case of TL, the relative alpha to beta response is found to be very different for each TL glow-peak, but it does not depend strongly on irradiation dose. In the case of LM – OSL measurements, it is found that the relative behaviour of the alpha to beta response is different for three distinct regions, namely the fast OSL component, the region of medium OSL component originating from the TL glow-peak at 110 °C when stimulation takes place at room temperature and finally the region of slow OSL component. Following stimulation at ambient temperature, the relative alpha to beta response of all components was not observed to depend significantly on dose, with the value of ratio being 0.03 and a tendency to decrease with increasing dose. However, in the case of measurements performed at 125 °C, the relative response of the fast components is much enhanced, and for the remaining components it increases with increasing dose. Special care must be taken to examine the relative alpha to beta response of the fast component at 125 °C which contrasts the relative response of the TL peak at ca. 325 °C. The implications for the dating of annealed quartz are also briefly discussed.     

The fast ratio: A rapid measure for testing the dominance of the fast component in the initial OSL signal from quartz

The signal from the fast component is usually considered preferable for quartz optically stimulated luminescence (OSL) dating, however its presence in a continuous wave (CW) OSL signal is often assumed, rather than verified. This paper presents an objective measure (termed the fast ratio) for testing the dominance of the fast component in the initial part of a quartz OSL signal. The ratio is based upon the photo ionisation cross-sections of the fast and medium components and the power of the measurement equipment used to record the OSL signal, and it compares parts of the OSL signal selected to represent the fast and medium components. The ability of the fast ratio to distinguish between samples whose CW-OSL signal is dominated by the fast and non-fast components is demonstrated by comparing the fast ratio with the contribution of the fast component calculated from curve deconvolution of measured OSL signals and from simulated data. The ratio offers a rapid method for screening a large number of OSL signals obtained for individual equivalent dose estimates, it can be calculated and applied as easily as other routine screening methods, and is transferrable between different aliquots, samples and measurement equipment.     

The dependence of quartz OSL on stimulation energy

Quartz is the mineral most commonly used for sediment dating. In dating practice, the optically stimulated luminescence (OSL) of quartz is measured mainly using the stimulation light whose wavelength is 470 ± 30 nm. The parameters of traps active in the OSL process are also determined for this stimulation band. The zeroing of the OSL is the fundamental condition of applicability of the luminescence dating for specific sediment and takes place in sunlight whose spectrum differs significantly from the band 470 ± 30 nm. In order to be able to know the course of OSL process in nature, a wider knowledge of the dependency of the trap parameters on the stimulation band is needed. Here the results are presented for the OSL measurements carried out with different wavelengths of stimulation light. For each stimulation band the components of the OSL signal are determined by the fitting procedure, and in this way the wavelength dependence of an individual component is found. The experiment has been repeated for two temperatures of OSL detection – the room temperature, which corresponds to natural conditions, and for 125 °C, which is the temperature usually applied for OSL measurement in dating. Four OSL components are presented in both experimental series. The values of their optical cross-section changes along with stimulation energy and temperature, as it is predicted by the model of OSL process including crystal lattice vibrations.     

Observations of thermal transfer OSL signals in glacigenic quartz

The conclusions of Rhodes and Pownall (Rhodes, E.J., Pownall, L., 1994. Zeroing of the OSL signal in quartz from young glaciofluvial sediments. Radiation Measurements 23, 329–333) were somewhat discouraging for the prospects of using quartz OSL for dating glacigenic sediments, while the more detailed study of Rhodes and Bailey (Rhodes, E.J., Bailey, R.M., 1997. The effect of thermal transfer on the zeroing of the luminescence of quartz from recent glaciofluvial sediments. Quaternary Science Reviews (Quaternary Geochronology) 16, 291–298) provided more encouragement. Specifically, the latter authors were able to account for the relatively high D_e values observed for recent glacigenic (dominantly glaciofluvial) sediments in terms of an anomalously high thermal transfer effect, rather than simply insufficient bleaching prior to deposition. In other locations, the OSL of quartz from glacigenic material appears to provide reliable age estimates, and does not suffer from these effects (Owen, L.A., Richards, B., Rhodes, E.J., Cunningham, W.D., Windley, B.F., Badamgarav, J., Dorjnamjaa, D., 1998. Relic permofrost structures in the Gobi of Mongolia: age and significance. Journal of Quaternary Science 13 (16), 539–548; Richards, B.W., Owen, L.A., Rhodes, E.J., 2000. Timing of Late Quaternary glaciations in the Himalayas of northern Pakistan. Journal of Quaternary Science 15, 283–297). In this paper, laboratory bleached samples from both the above studies are remeasured, using an experimental design to correct for OSL sensitivity changes, which has some similarities to the single aliquot regenerative dose (SAR) protocol of Murray and Wintle (Murray A.S., Wintle A.G., 2000. Luminescence dating of quartz using an improved single-aliquot regenerative-dose protocol. Radiation Measurements 32, 57–73). Clear evidence of thermal transfer OSL signals, generated during the preheating procedure, is presented. Further measurements, using the full SAR protocol, demonstrate that the source of this charge is related to natural dosing. For one sample, the apparent effect is subtracted effectively by the SAR protocol. Another sample studied in detail shows a striking relationship between the thermally transferred OSL signal and the total TL observed during the ramping of the preceding preheat treatment.     

Zeroing of the OSL signal in quartz from young glaciofluvial sediments

The natural luminescence of quartz samples from recent (<200 yr old) glaciofluvial sediments collected from a range of distances from the snout of the Gangotri glacier in the Garhwal Himalaya, India, was measured. Six measured D_E (equivalent dose) values ranged from 35 to 175 Gy, strongly suggesting that these samples had been exposed to daylight only poorly before deposition. However, regenerated growth curves constructed after exposure to several hours of natural daylight gave apparent D_E values ranging from 10 to 30 Gy. Detailed measurements of one sample confirm that these observations are due to a huge recuperation effect. The “shine plateaux” observed in the majority of these D_E determinations showed little increase of D_E with increasing exposure time. The mechanisms of this unexpected behaviour, and the implications for the detection of partial bleaching, are discussed.     

The timing of OSL sensitivity changes in a natural quartz

The timing of 110°C thermoluminescence (TL) and optically stimulated luminescence (OSL) sensitivity changes is explored using a natural (aeolian) quartz sample from Australia that was previously found to exhibit marked dose-dependent sensitivity change. The changes occur asynchronously; the 110°C TL sensitivity changes after dosing plus pre-heating, whereas the OSL sensitivity changes (proportionately with dose) after optical bleaching. Although the magnitude and saturation characteristics of the sensitivity changes are found to be similar, their non-synchronicity negates a direct link between the phenomena. Implications of these results for dating procedures are discussed. In particular, the results indicate that a single aliquot additive dose procedure similar to that developed for coarse-grained potassium feldspar should be possible for some quartz samples.     

Analysis of optical bleaching of OSL signal in sediment quartz

The aim of this work was to study the effect of the quality of optical bleaching on the results of OSL (Optically Stimulated Luminescence) dating method. The large aliquots of coarse quartz grains extracted from fluvial deposit were used in the study. The poor, medium and good bleaching were simulated in laboratory with help of Blue LED light source in series of experiments. Then the samples were irradiated with a common laboratory dose. The equivalent doses (DE) were measured by the help of standard Single Aliquot Regeneration (SAR) technique, but obtained DE distributions are analyzed in a new way. The method for recognizing and compensating for partial bleaching is proposed. The conclusions for dating sediment quartz samples are presented and discussed.     

Application of pulsed OSL to polymineral fine-grained samples

Pulsed OSL is applied to nine fine-grained sediment samples from Sichuan province, China, using stimulating pulses of 10 μs on and 240 μs off, with an infrared exposure prior to each OSL measurement. Comparison of fading rates between pulsed and non-pulsed signals, the latter also obtained with a preceding IR exposure, shows that fading is significant for mainly the non-pulsed signals. Presence of a pulsed IRSL and the magnitudes of b-value to correct for lower alpha efficiency suggest that pulsing does not fully remove a significant feldspar signal, only a fading component. Comparison with ages of quartz extracts shows that pulsed OSL ages are consistent, while CW-OSL ages are slightly older and CW-IRSL ages are much older. The older ages suggest a less well-bleached feldspar component.     

Applicability of OSL pre-dose phenomenon of quartz in the estimation of equivalent dose

The feasibility of utilizing the pre-dosed OSL signal in the estimation of the equivalent dose has been investigated. The results based on (i) the behavior of growth curve, (ii) dose recovery tests and (iii) non-bleachability of reservoir centres, R-centres, suggests that (i) the pre-dosed OSL does not seem to work satisfactorily in dose estimation unlike the pre-dosed 110 °C TL emission and (ii) it may not be applicable in case of bleached specimen.     

The dose dependency of the over-dispersion of quartz OSL single grain dose distributions

The use of single grain quartz OSL dating has become widespread over the past decade, particularly with application to samples likely to have been incompletely bleached before burial. By reducing the aliquot size to a single grain the probability of identifying the grain population most likely to have been well-bleached at deposition is maximised and thus the accuracy with which the equivalent dose can be determined is – at least in principle – improved.However, analysis of single grain dose distributions requires knowledge of the dispersion of the well-bleached part of the dose distribution. This can be estimated by measurement of a suitable analogue, e.g. a well-bleached aeolian sample, but this requires such an analogue to be available, and in addition the assumptions that the sample is in fact a) well-bleached, and b) has a similar dose rate heterogeneity to the fossil deposit. Finally, it is an implicit assumption in such analysis that any over-dispersion is not significantly dose dependent.In this study we have undertaken laboratory investigations of the dose dependency of over-dispersion using a well-bleached modern sample with an average measured dose of 36 ± 3 mGy. This sample was prepared as heated (750 °C for 1 h), bleached and untreated portions which were then given uniform gamma doses ranging from 100 mGy to 208 Gy. We show that for these samples the relative laboratory over-dispersion is not constant as a function of dose and that the over-dispersion is smaller in heated samples. We also show that the dim grains in the distributions have a greater over-dispersion than the bright grains, implying that insensitive samples will have greater values of over-dispersion than sensitive samples.     

Changes in OSL properties of quartz by preheating: an interpretation

A study of OSL variation with preheat temperature showed, in a majority of cases, that OSL recorded at room temperature, increases above 200°C before the normal drainage at higher temperature. To explain this behaviour, an alternative interpretation to the common ‘electronic thermal transfer’ mechanism is suggested, supported by a study of hydrothermally grown quartz crystals. This interpretation involves impurities in substitution of Si⁴⁺, specially Al³⁺, which are associated with species like, in the case of quartz, hydrogen (H⁺, in fact, OH⁻) and alkali ions (Li⁺, Na⁺, K⁺). These monovalent ions usually act as charge compensators and are mobile during heating. As a consequence of the mobility and a possible irreversible exchange between compensators, the number of radiative recombination centres associated with the OSL trap(s), observable within the detection spectral window used (250–400 nm), increases during preheating. This phenomenon could lead to a wrong ED determination.     

Investigations into the reliability of SAR-OSL equivalent doses obtained for quartz samples displaying dose response curves with more than one component

Fast component dominated quartz single aliquot regenerative dose optically stimulated luminescence (SAR-OSL) dose response curves that display continuing growth at high doses are increasingly reported in literature. This behaviour would result in higher equivalent doses being obtained. Here we document the characteristics of OSL signals from fine (4–11 μm) and coarse (63–90 μm) quartz extracted from Romanian loess that display such behaviour. For very high doses (>1 kGy up to 5–15 kGy) the data could be closely fitted to a double saturating exponential regression model. Nonetheless, the saturation charcteristics of these fine and coarse quartz grains are very different, with average saturation chracteristic doses of D₀₁ ≈ 175 Gy and D₀₂ ≈ 1800 Gy in the case of the fine material, while in the case of the coarse material values of D₀₁ ≈ 55 Gy and D₀₂ ≈ 600 Gy have been obtained. Our results imply a hitherto unexplained mechanism in OSL production at high doses and question the reliability of obtaining SAR-OSL equivalent doses in the high dose region when a second function is needed to describe the dose response.     

Assessing the impact of pulsed-irradiation procedures on the thermally transferred OSL signal in quartz

Thermally transferred optically stimulated luminescence (TT-OSL) dating protocols have been suggested as a means of extending the age range of luminescence dating. Several studies demonstrate that TT-OSL signals increase with large radiation doses (>2000 Gy) and yet, few studies report older TT-OSL ages (>400 Gy) in agreement with independent absolute age control. In one such study, agreement with independent chronology was only achieved for the old samples by implementing a pulsed-irradiation procedure. Pulsed-irradiation is suggested to compensate for dose rate dependent competition effects by dividing the laboratory irradiation into discrete irradiation steps interspersed with heat treatments. However, every inter-step heat treatment has the potential to anneal part of the TT-OSL dating signal. This study compares constant- and pulsed-irradiation TT-OSL protocols and investigates the degree of partial thermal annealing. The results suggest that almost all of the difference in outcome between constant- and pulsed-irradiation protocols can be explained by partial annealing of the TT-OSL signal rather than by competition effects. Partial annealing distorts the laboratory dose response curve but has no impact on the natural signal, resulting in unreliable equivalent dose estimates. This means that pulsed-irradiation procedures may not be viable for TT-OSL dating measurements. Future studies implementing pulsed-irradiation procedures should carefully consider the extent to which inter-step thermal treatments partially anneal the signal.     

Testing the accuracy of a Bayesian central-dose model for single-grain OSL,using known-age samples

While reviews of comparisons between multi-grain OSL ages and independent chronological information are available in the literature, there is hardly any such performance test for single-grain OSL ages. And yet, this is all the more needed as the interpretation of single-grain dose distributions remains a difficult task, given the typically considerable dispersion in equivalent dose values measured by OSL – and the numerous sources of such dispersion in measurements. Here, we present the study of 19 samples for which independent age control is available, and whose ages range from 2 to 46 ka. Based on multi-grain OSL age estimates, these samples are presumed to have been both well-bleached at burial, and unaffected by mixing after deposition. Two ways of estimating single-grain ages are then compared: the standard approach on the one hand, consisting of applying the Central Age Model to D_e values determined with the Analyst software; on the other hand, the central dose model recently proposed by Combès et al. (Combès, B., Philippe, A., Lanos, P., Mercier, N., Tribolo, C., Guerin, G., Guibert, P., Lahaye, C., in press. Quaternary Geochronology). The median of the relative discrepancy between single-grain OSL and reference ages is about twice as large for the standard approach (12%) as with the Bayesian model (7%). Statistical tests show that, based on our (limited) dataset, the difference between the two models seems to be significant for samples in the age range 4–46 ka. Finally, the influence of various factors on the (in-)accuracy of single grain OSL ages is discussed; it appears that the accuracy of ages estimated in a standard way decreases when age is increased, while the Bayesian model seems more robust. This study also shows that (i) there is no 20% limit on the CAM overdispersion parameter for well-bleached samples; (ii) dose recovery experiments do not seem to be a very reliable tool to estimate the accuracy of a SAR measurement protocol for age determination.     

Assessing the impact of IR stimulation at increasing temperatures to the OSL signal of contaminated quartz

The purpose of the present study is to identify the effect of the increasing temperature IR stimulation to the component-resolved OSL luminescence signal of mixed quartz-feldspars material. Post IR OSL signals measured at 110 °C were analysed via only general order kinetic terms, while IR signals obtained at increasing temperatures were de-convolved using the sum of general order kinetics plus a tunnelling component. By increasing stimulation temperature, it was demonstrated that IRSL at temperatures above 50 °C does not only stimulate feldspar but also stimulates both fast and medium quartz OSL components. In the temperature range between 175 and 250 °C, the IRSL initial intensity is dominated by the fast OSL component. Estimated equivalent doses using either Post-IR₁₇₅.OSL₁₁₀ as well as IRSL₁₇₅ (with the indices indicating the measurement temperature) are in good agreement between each other, due to both stimulating quartz. Finally, the physical meaningfulness of the fitting parameters for the tunnelling component is also discussed.